Near-threshold H/D exchange in CD3CHO photodissociation

Nature Chemistry

Volumn 3, Issue 6, 2011, Pages 443-448

  Heazlewood, Brianna R ^a   MacCarone, Alan T ^a   Andrews, Duncan U ^a   Osborn, David L ^b   Harding, Lawrence B ^c   Klippenstein, Stephen J ^c   Jordan, Meredith J T ^a   Kable, Scott H ^a  

^a UNIVERSITY OF SYDNEY   (Australia)

^b SANDIA NATIONAL LABORATORIES   (United States)

^c ARGONNE NATIONAL LABORATORY   (United States)

Author keywords

[No Author keywords available]

Indexed keywords

DEUTERIUM; HYDROGEN;

ARTICLE; CHEMISTRY; PHOTOCHEMISTRY;

DEUTERIUM; HYDROGEN; PHOTOCHEMISTRY;

EID: 79957494935     PISSN: 17554330     EISSN: 17554349     Source Type: Journal    
DOI: 10.1038/nchem.1052     Document Type: Article

References (41)

1. Urey, H. C., Brickwedde, F. G. & Murphy, G. M. A hydrogen isotope of mass 2. Phys. Rev. 39, 164-165 (1932).
2. Jefferts, K. B., Penzias, A. A. & Wilson, R. W. Deuterium in the Orion nebula. Astrophys. J. 179, L57-L59 (1973).
3. Gourier, D. et al. Extreme deuterium enrichment of organic radicals in the Orgueil meteorite: revisiting the interstellar interpretation? Geochim. Cosmochim. Acta 72, 1914-1923 (2008).
4. Feng, X. H. & Epstein, S. Climatic implications of an 8000-year hydrogen isotope time-series from bristlecone-pine trees. Science 265, 1079-1081 (1994). (Pubitemid 24293830)
5. Zhang, X. N., Gillespie, A. L. & Sessions, A. L. Large D/H variations in bacterial lipids reflect central metabolic pathways. Proc. Natl Acad. Sci. USA 106, 12580-12586 (2009).
6. Kaye, J. A. in Isotope Effects in Gas-Phase Chemistry (ed. Kaye, J. A.) Ch. 1, 1-14 (American Chemical Society, 1992).
7. Konermann, L., Tong, X. & Pan, Y. Protein structure and dynamics studied by mass spectrometry: H/D exchange, hydroxyl radical labeling, and related approaches. J. Mass Spectrom. 43, 1021-1036 (2008).
8. Shirota, T., Mano, N., Tsuge, M. & Hoshina, K. Formation of H3O+ from alcohols and ethers induced by intense laser fields. Rapid Comm. Mass Spec. 24, 679-686 (2010).
9. van Raalte, D. & Harrison, A. G. Energetics and mechanism of hydronium ion formation by electron impact. Can. J. Chem. 41, 3118-3125 (1963).
10. Qadiri, R. H., Feltham, E. J., Nahler, N. H., Garcia, R. P. & Ashfold, M. N. R. Propyne and allene photolysis at 193.3 nm and at 121.6 nm. J. Chem. Phys. 119, 12842-12851 (2003).
11. Ganot, Y., Rosenwaks, S. & Bar, I. H and D release in 243.1 nm photolysis of vibrationally excited 3n1, 4n1, and 4nCD overtones of propyne-d3. J. Chem. Phys. 120, 8600-8607 (2004).
12. Robinson, J. C., Sveum, N. E., Goncher, S. J. & Neumark, D. M. Photofragment translational spectroscopy of allene, propyne and propyne-d3 at 193 nm. Mol. Phys. 103, 1765-1783 (2005). (Pubitemid 41673110)
13. Lin, C-K. et al. Photoisomerization and photodissociation of toluene in a molecular beam. J. Am. Chem. Soc. 124, 4068-4075 (2002). (Pubitemid 34310920)
14. Huang, C-L., Jiang, J-C., Lee, Y. T. & Ni, C-K. Photoisomerization and photodissociation of m-xylene in a molecular beam. J. Phys. Chem. A 107, 4019-4024 (2003).
15. Lee, S-H., Lee, Y. T. & Yang, X. Dynamics of photodissociation of ethylene and its isotopomers at 157 nm: branching ratios and kinetic-energy distributions. J. Chem. Phys. 120, 10983-10991 (2004).
16. Lee, S-H., Lee, Y. T. & Yang, X. Dynamics of photodissociation of 3,3,3-d3-propene at 157 nm: site effect and hydrogen migration. J. Chem. Phys. 120, 10992-10999 (2004).
17. Deyerl, H-J., Fischer, I. & Chen, P. Photodissociation dynamics of the allyl radical. J. Chem. Phys. 110, 1450-1461 (1999).
18. Deyerl, H-J., Fischer, I. & Chen, P. Photodissociation dynamics of the propargyl radical. J. Chem. Phys. 111, 3441-3448 (1999).
19. Schinke, R. Photodissociation Dynamics (Cambridge Univ. Press, 1993).
20. Reid, S. A. & Reisler, H. Experimental studies of resonances in unimolecular decomposition. Annu. Rev. Phys. Chem. 47, 495-525 (1996). (Pubitemid 126416973)
21. Townsend, D. et al. The roaming atom: straying from the reaction path in formaldehyde decomposition. Science 306, 1158-1161 (2004). (Pubitemid 39488989)
22. Houston, P. L. & Kable, S. H. Photodissociation of acetaldehyde as a second example of the roaming mechanism. Proc. Natl Acad. Sci. USA 103, 16079-16082 (2006). (Pubitemid 44715154)
23. Heazlewood, B. R. et al. Roaming dynamics: the dominant pathway to molecular products in acetaldehyde photodissociation. Proc. Natl Acad. Sci. USA 105, 12719-12724 (2008).
24. Suits, A. G. Roaming atoms and radicals: a new mechanism in molecular dissociation. Acc. Chem. Res. 41, 873-881 (2008).
25. Harding, L. B., Georgievskii, Y. & Klippenstein, S. J. Roaming radical kinetics in the decomposition of acetaldehyde. J. Phys. Chem. A 114, 765-777 (2010).
26. Shepler, B. C., Braams, B. J. & Bowman, J. M. Quasiclassical trajectory calculations of acetaldehyde dissociation on a global potential energy surface indicate significant non-transition state dynamics. J. Phys. Chem. A 111, 8282-8285 (2007). (Pubitemid 47387978)
27. Sivaramakrishnan, R., Michael, J. V. & Klippenstein, S. J. Direct observation of roaming radicals in the thermal decomposition of acetaldehyde. J. Phys. Chem. A 114, 755-764 (2010).
28. Heazlewood, B. R., Rowling, S. J., Maccarone, A. T., Jordan, M. J. T. & Kable, S. H. Photochemical formation of HCO and CH3 on the ground S0 (1AŒ) state of CH3CHO. J. Chem. Phys. 130, 054310 (2009).
29. Thompson, K. C., Crittenden, D. L., Kable, S. H. & Jordan, M. J. T. A classical trajectory study of the photodissociation dynamics of T1 acetaldehyde: the transition from impulsive to statistical dynamics. J. Chem. Phys. 124, 044302 (2006).
30. Gherman, B. F., Friesner, R. A., Wong, T-H., Min, Z. & Bersohn, R. Photodissociation of acetaldehyde: the CH4 + CO channel. J. Chem. Phys. 114, 6128-6133 (2001).
31. Lee, S-H. & Chen, I-C. Axis switching in theB∼ 2AŒ-X∼ 2AŒ transition of HCO and fluorescence lifetimes of the B∼ 2AŒ(0,0,0) rotational states. J. Chem. Phys. 105, 2583-2590 (1996).
32. Gripp, J., Kuczmann, A., Stöck, C., Temps, F. & Tröllsch, A. The (B∼ 2AŒ-X∼ 2AŒ) laser induced fluorescence excitation spectrum of DCO in a supersonic jet expansion. Phys. Chem. Chem. Phys. 2, 1653-1657 (2000).
33. Rowling, S. J. Competing Electronic States in Formaldehyde Dissociation, Ch. 7. PhD thesis, Univ. Sydney (2010).
34. Yadav, J. S. & Goddard, J. D. Acetaldehyde photochemistry - the radical and molecular dissociations. J. Chem. Phys. 84, 2682-2690 (1986).
35. Amaral, G. A., Arregui, A., Rubio-Lago, L., Rodríguez, J. D. & Ban∼ares, L. Imaging the radical channel in acetaldehyde photodissociation: competing mechanisms at energies close to the triplet exit barrier. J. Chem. Phys. 133, 064303 (2010).
36. Lee, S-H. & Chen, I-C. Photofragments CH3(X∼ 2A2 ŒŒ)+HCO(X∼ 2AŒ) from acetaldehyde: distributions of rotational states and preferential population of K doublets of HCO. J. Chem. Phys. 105, 4597-4604 (1996). (Pubitemid 126747830)
37. Yang, X., Maeda, S. & Ohno, K. Insight into global reaction mechanism of [C2, H4, O] system from ab initio calculations by the scaled hypersphere search method. J. Phys. Chem. A 111, 5099-5110 (2007). (Pubitemid 47012624)
38. Nguyen, T. L., Vereecken, L., Hou, X. J., Nguyen, M. T. & Peeters, J. Potential energy surfaces, product distributions and thermal rate coefficients of the reaction of O(3P) with C2H4 (X∼ 1Ag): a comprehensive theoretical study. J. Phys. Chem. A 109, 7489-7499 (2005).
39. Harding, L. B., Klippenstein, S. J. & Jasper, A. W. Ab initio methods for reactive potential surfaces. Phys. Chem. Chem. Phys. 9, 4055-4070 (2007).
40. Finlayson-Pitts, B. J. and Pitts, J. N. Jr Chemistry of the Upper and Lower Atmosphere - Theory, Experiments, and Applications (Academic Press, 1999).
41. Terentis, A. C., Stone, M. & Kable, S. H. Dynamics of acetaldehyde dissociation at 308 nm: rotational (N, Ka) and translational distributions of the HCO photoproduct. J. Phys. Chem. 98, 10802-10808 (1994).